Understanding the effects of diffusion coefficient and exchange current density on the electrochemical model of lithium-ion batteries

Lee, Hyobin; Yang, Seungwon; Kim, Suhwan; Song, Jihun; Park, Joonam; Doh, Chil‐Hoon; Ha, Yoon‐Cheol; Kwon, Tae-Young; Lee, Yongmin

doi:10.1016/j.coelec.2022.100986

Cited by 23 publications

(19 citation statements)

References 112 publications

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“…To obtain these results, we assume that the radius (r) parameter in equations (1-2) equals the radius of the secondary particle measured by SEM, as generally assumed in this field 6,7,10,40 . Consistent with previous works 6,7,22,32,39,[41][42][43][44][45] , j0 increases with more lithium extraction (higher SOC). The range of obtained values for j0 (0.01 to 0.1 mA cm -2 ) and DLi (10 -10 to10 -9 cm 2 s -1 ) are broadly consistent with previous reports of polycrystalline NMC particles taken at both the porous electrode 32,39,41-45 and single-particle 6,7,22 levels (Fig.…”

Section: Quantification Of Exchange Current Density and Lithium Diffu...supporting

confidence: 91%

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Min

Gubow

Hargrave

et al. 2023

Preprint

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Polycrystalline Li(Ni,Mn,Co)O2 (NMC) secondary particles are the most common cathode materials for Li-ion batteries. During electrochemical (dis)charge, lithium is believed to diffuse through the bulk and enter (leave) the secondary particle at the surface. Based on this model, smaller particles would cycle faster due to shorter diffusion lengths and larger surface-area-to-volume ratios. In this work, we evaluate this widespread assumption by developing a new high-throughput single-particle electrochemistry platform using the multi-electrode array from neuroscience. By measuring the reaction and diffusion times for 21 individual particles in liquid electrolytes, we find no correlation between the particle size and either the reaction or diffusion times, which is in stark contrast to the prevailing lithium transport model. We propose that electrochemical reactions occur inside secondary particles, possibly due to electrolyte penetration into cracks. Our high-throughput, single-particle electrochemical platform further opens new frontiers for robust, statistical quantification of individual particles in electrochemical systems.

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Section: Quantification Of Exchange Current Density and Lithium Diffu...supporting

confidence: 91%

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Min

Gubow

Hargrave

et al. 2023

Preprint

View full text Add to dashboard Cite

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“…In addition, straight lines having a phase of approximately 45° can be observed at relatively low frequencies at each SOC and DOD, and these correspond to the Warburg impedance arising from the diffusion of electroactive species. The impedance ( Z ) of semi-infinite diffusion in a film electrode can be expressed using eqs and . , …”

Section: Resultsmentioning

confidence: 99%

“…The impedance (Z) of semi-infinite diffusion in a film electrode can be expressed using eqs 1 and 2. 31,32…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Fujita

Hakari

Sakuda

et al. 2022

ACS Appl. Energy Mater.

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Lithium sulfur (Li/S) batteries are promising next-generation battery candidates owing to their high energy densities. In particular, the fast solid-state S/Li2S redox reactions are crucial to increase the energy density and extend the cycle life of such batteries. However, the poor electronic and ionic conductivities of S and Li2S result in a low reversible capacity. Therefore, an electrode design is required to achieve high-energy-density Li/S batteries. In this study, we investigated the charge–discharge mechanism of a solid solution of Li2S and LiI (Li2S–LiI) in all-solid-state batteries showing excellent electrochemical properties, including cycling performance. We found that a high reversible capacity was achieved despite the high conversion of Li2S into S because the ionic conductivity of the positive electrode was maintained during charging and discharging, and this was a result of the formation of an ionic conductive structure comprising LiI-rich domains. Crucially, essentially fully solid phase S/Li2S reactions in all-solid-state batteries were attained by fully eliminating the sulfide solid electrolyte from the positive electrode. These findings enable the design of S- and Li2S-based positive electrodes for solid phase redox reactions for use in high-energy-density Li/S batteries.

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“…It excludes the active surface area and voltage plateau effects and is well-suited for analyzing the electrochemical reaction kinetics of LiFePO 4 , which has a flat voltage plateau. 23 Therefore, the relationship between the Li + diffusion coefficient and electrode potential was investigated using PITT to record current variations over time in a series of potential steps. The diffusion lengths and slopes of the linear regions of plots of ln(I t ) versus time were used to determine the potential-dependent Li + diffusion coefficients (Figure 4a).…”

mentioning

confidence: 99%

“…PITT is a powerful technique for studying Li + diffusivity. It excludes the active surface area and voltage plateau effects and is well-suited for analyzing the electrochemical reaction kinetics of LiFePO 4 , which has a flat voltage plateau . Therefore, the relationship between the Li + diffusion coefficient and electrode potential was investigated using PITT to record current variations over time in a series of potential steps.…”

mentioning

confidence: 99%

Tannic Acid-Derived Carbon Coating on LiFePO₄ Nanocrystals Enables High-Rate Cathode Materials for Lithium-Ion Batteries

Wang

Cui

Cheng

et al. 2023

ACS Appl. Nano Mater.

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Tannic acid (TA) is a plant polyphenol capable of coating hydrothermally grown LiFePO 4 nanocrystals by simple wet impregnation and drying. Mild pyrolysis in an inert atmosphere transforms the TA coating on LiFePO 4 nanocrystals into homogeneous and compact carbon films. Introducing conductive carbon films on LiFePO 4 nanocrystals increases the electrical conductivity of the LiFePO 4 /C composite. However, reaction kinetics revealed that excessively thick carbon films limit the Li + diffusivity of the LiFePO 4 /C composite during delithiation/lithiation. Therefore, the electrical conductivity and Li + diffusivity must be balanced to achieve the required electrochemical properties.

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Understanding the effects of diffusion coefficient and exchange current density on the electrochemical model of lithium-ion batteries

Cited by 23 publications

References 112 publications

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Tannic Acid-Derived Carbon Coating on LiFePO₄ Nanocrystals Enables High-Rate Cathode Materials for Lithium-Ion Batteries

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Understanding the effects of diffusion coefficient and exchange current density on the electrochemical model of lithium-ion batteries

Cited by 23 publications

References 112 publications

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Direct measurements of size-independent lithium diffusion and reaction times in individual polycrystalline battery particles

Li2S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Tannic Acid-Derived Carbon Coating on LiFePO4 Nanocrystals Enables High-Rate Cathode Materials for Lithium-Ion Batteries

Contact Info

Product

Resources

About

Li₂S–LiI Solid Solutions with Ionic Conductive Domains for Enhanced All-Solid-State Li/S Batteries

Tannic Acid-Derived Carbon Coating on LiFePO₄ Nanocrystals Enables High-Rate Cathode Materials for Lithium-Ion Batteries